多功能分離介質(zhì)的合成和應(yīng)用
發(fā)布時間：2018-07-21 16:32
【摘要】：分離科學(xué)是自然科學(xué)中很重要的一個研究方向。近年來,隨著食品科學(xué)、生物醫(yī)藥、環(huán)境科學(xué)、化工生產(chǎn)等學(xué)科的快速發(fā)展,對這些行業(yè)中相關(guān)目標分析物的分離和純化提出了更高的要求�；诖�,各種分離純化方法得到了快速發(fā)展。高效液相色譜法(High performance liquid chromatography, HPLC)作為經(jīng)典的分離方法,是分離各類化合物的重要選擇。而磁固相萃取(Magnetic solid phase extraction, MSPE)相較于傳統(tǒng)固相萃取(Solid phase extraction, SPE),具有操作簡單、快速高效等優(yōu)點,近年來也得到了迅速發(fā)展。分離方法的核心是分離介質(zhì)。為了提高分離介質(zhì)的分離效果,新型分離介質(zhì)的合成一直是分離科學(xué)中最有活力的工作。由于實際樣品分析中樣品的多樣性和復(fù)雜性,新型分離介質(zhì)的設(shè)計必須結(jié)合實際樣品分離分析的需要,所合成的分離介質(zhì)除了對目標分析物要有很好的選擇性之外,還要具有優(yōu)秀的穩(wěn)定性、重現(xiàn)性以及實際可操作性。除此之外,新型分離介質(zhì)的合成要盡可能操作簡單,制備周期短,以及經(jīng)濟環(huán)保。鑒于此,本論文開發(fā)了多種新的分離介質(zhì)合成方法,所提出的合成方法操作簡單實用、普適性高、重現(xiàn)性好�；谒_發(fā)的合成方法制備了一系列新型分離介質(zhì),包括一種混合模式硅膠基質(zhì)填充柱,兩種混合模式毛細管整體柱,以及兩種磁分離材料,并將這些新型分離介質(zhì)應(yīng)用于不同類別分析物的分離,取得了很好的效果。具體內(nèi)容如下所示：一、將RAFT/click chemistry串聯(lián)接枝法應(yīng)用于聚合物接枝色譜固定相的合成,基于此方法合成了一種內(nèi)嵌酰胺基聚苯乙烯接枝的反相弱陰離子交換(Reverse phase/weak anionic exchange chromatography, RP/WAX)硅膠固定相,所制固定相展現(xiàn)出很好的硅羥基屏蔽效果,在純水做流動相時穩(wěn)定性良好。二、將雙鍵改性POM作為新的功能單體,利用共聚法制備了一種新的POM修飾聚合物整體柱。加入POM后制備的整體柱具有強陽離子交換性質(zhì),柱效和滲透性得到了明顯的提升,對于極性帶電化合物展現(xiàn)出很好的分離效果。三、開發(fā)了一種新的“一鍋法”用來制備混合模式有機-硅膠雜化整體柱�；诖朔椒�,我們制備了一種鍵合有辛基和膦酸基的反相陽離子交換(Reverse phase/cationic exchange chromatography, RP/CEC)有機-硅膠雜化整體柱。以此整體柱為分離柱構(gòu)建了納升液相色譜-質(zhì)譜聯(lián)用(Nanoliter-liquid chromatography-mass spectrometry, nano-LC-MS)平臺,結(jié)合移液槍頭固相萃取(Pipette tip-solid phase extraction, PT-SPE)與衍生化方法,對5 mg水稻葉片中的內(nèi)源性赤霉素進行了定量分析。四、成功的在納米Fe3O4表面固載納米線結(jié)構(gòu)的鈦-甘油(Titanium-glycerol, TiGly)復(fù)合物或鋯-甘油復(fù)合物(Zirconium-glycerol, ZrGly),所合成的Fe3O4@TiGly和Fe3O4@ZrGly形貌均一,比表面明顯提高。在MSPE模式下,將這兩種材料應(yīng)用于生物體液中核糖核苷和磷酸化多肽的萃取。結(jié)果表明Fe3O4@ZrGly對核糖核苷具有更好的富集純化效果,而Fe3O4@TiGly對磷酸化多肽具有更好的富集純化效果。
[Abstract]:Separation science is a very important research direction in natural science. In recent years, with the rapid development of food science, biological medicine, environmental science, chemical production and other disciplines, the separation and purification of related target analytes in these industries is higher. Based on this, various separation and purification methods have been developed rapidly. High performance liquid chromatography (HPLC), as a classic separation method, is an important choice for the separation of all kinds of compounds. The magnetic solid phase extraction (Magnetic solid phase extraction, MSPE) has the advantages of simple operation, fast efficiency and so on. In recent years, the phase of Magnetic solid phase extraction (MSPE) has the advantages of simple operation, rapid and efficient. The core of the separation method is the separation medium. In order to improve the separation effect of the separation medium, the synthesis of the new separation medium has been the most active work in the separation science. Because of the diversity and complexity of the samples in the actual sample analysis, the design of the new separation medium must be combined with the needs of the actual sample separation and analysis. In addition to the excellent stability, reproducibility and practical maneuverability of the synthesized separation medium, in addition to the good selectivity of the target analyte, the synthesis of the new separation medium should be simply operated, the preparation period is short, and the economic ring is guaranteed. In view of this, this paper has developed a variety of new separation media. The synthetic method is simple and practical, high universality and good reproducibility. A series of new separation mediums are prepared based on the synthetic method developed, including a mixed mode silica gel matrix filling column, two mixed mode capillary monolithic columns, and two magnetic separation materials, and the new separation medium is applied to the new separation medium. The separation of different types of analytes has achieved good results. The specific contents are as follows: first, the RAFT/click Chemistry Series grafting method is applied to the synthesis of polymer graft chromatography stationary phase, and a kind of Reverse phase/weak anionic exchang graft with embedded amidyl polystyrene (phase/weak anionic exchang) is synthesized by this method. E chromatography, RP/WAX) silica gel fixed phase, the fixed phase showed a good silicon hydroxyl shielding effect, in pure water as a mobile phase stability. Two, the double bond modified POM as a new functional monomer, the use of copolymerization to prepare a new POM modified polymer monolithic column. The whole column after the addition of POM has strong cation exchange. A new kind of "one pot method" was developed for the preparation of mixed mode organic silica hybrid monolithic column. Based on this method, a kind of reverse phase cation exchange (Revers) bonded with octyl and phosphonic acid (Revers) was prepared. E phase/cationic exchange chromatography, RP/CEC) organic silica gel hybrid monolithic column. A Nanoliter-liquid chromatography-mass spectrometry (nano-LC-MS) platform was constructed by using the monolithic column as separation column, and the solid phase extraction (Pipette tip-solid phase) and derivatization were combined with the pipette. The quantitative analysis of endogenous gibberellin in 5 mg rice leaves was made. Four, successfully loaded nanowires on the surface of nanoscale Fe3O4 (Titanium-glycerol, TiGly) complex or zirconium glycerol complex (Zirconium-glycerol, ZrGly), the morphology of the synthesized Fe3O4@TiGly and Fe3O4@ZrGly was homogeneous, and the surface was significantly higher than that of the surface. In MSPE model, these two kinds of materials were applied to the extraction of ribonucleoside and phosphorylated polypeptide in biological fluid. The results showed that Fe3O4@ZrGly had better enrichment and purification effect on ribonucleoside, while Fe3O4@TiGly had better enrichment and purification effect on phosphorylated polypeptide.
【學(xué)位授予單位】：武漢大學(xué)
【學(xué)位級別】：博士
【學(xué)位授予年份】：2016
【分類號】：TQ028
[Abstract]:Separation science is a very important research direction in natural science. In recent years, with the rapid development of food science, biological medicine, environmental science, chemical production and other disciplines, the separation and purification of related target analytes in these industries is higher. Based on this, various separation and purification methods have been developed rapidly. High performance liquid chromatography (HPLC), as a classic separation method, is an important choice for the separation of all kinds of compounds. The magnetic solid phase extraction (Magnetic solid phase extraction, MSPE) has the advantages of simple operation, fast efficiency and so on. In recent years, the phase of Magnetic solid phase extraction (MSPE) has the advantages of simple operation, rapid and efficient. The core of the separation method is the separation medium. In order to improve the separation effect of the separation medium, the synthesis of the new separation medium has been the most active work in the separation science. Because of the diversity and complexity of the samples in the actual sample analysis, the design of the new separation medium must be combined with the needs of the actual sample separation and analysis. In addition to the excellent stability, reproducibility and practical maneuverability of the synthesized separation medium, in addition to the good selectivity of the target analyte, the synthesis of the new separation medium should be simply operated, the preparation period is short, and the economic ring is guaranteed. In view of this, this paper has developed a variety of new separation media. The synthetic method is simple and practical, high universality and good reproducibility. A series of new separation mediums are prepared based on the synthetic method developed, including a mixed mode silica gel matrix filling column, two mixed mode capillary monolithic columns, and two magnetic separation materials, and the new separation medium is applied to the new separation medium. The separation of different types of analytes has achieved good results. The specific contents are as follows: first, the RAFT/click Chemistry Series grafting method is applied to the synthesis of polymer graft chromatography stationary phase, and a kind of Reverse phase/weak anionic exchang graft with embedded amidyl polystyrene (phase/weak anionic exchang) is synthesized by this method. E chromatography, RP/WAX) silica gel fixed phase, the fixed phase showed a good silicon hydroxyl shielding effect, in pure water as a mobile phase stability. Two, the double bond modified POM as a new functional monomer, the use of copolymerization to prepare a new POM modified polymer monolithic column. The whole column after the addition of POM has strong cation exchange. A new kind of "one pot method" was developed for the preparation of mixed mode organic silica hybrid monolithic column. Based on this method, a kind of reverse phase cation exchange (Revers) bonded with octyl and phosphonic acid (Revers) was prepared. E phase/cationic exchange chromatography, RP/CEC) organic silica gel hybrid monolithic column. A Nanoliter-liquid chromatography-mass spectrometry (nano-LC-MS) platform was constructed by using the monolithic column as separation column, and the solid phase extraction (Pipette tip-solid phase) and derivatization were combined with the pipette. The quantitative analysis of endogenous gibberellin in 5 mg rice leaves was made. Four, successfully loaded nanowires on the surface of nanoscale Fe3O4 (Titanium-glycerol, TiGly) complex or zirconium glycerol complex (Zirconium-glycerol, ZrGly), the morphology of the synthesized Fe3O4@TiGly and Fe3O4@ZrGly was homogeneous, and the surface was significantly higher than that of the surface. In MSPE model, these two kinds of materials were applied to the extraction of ribonucleoside and phosphorylated polypeptide in biological fluid. The results showed that Fe3O4@ZrGly had better enrichment and purification effect on ribonucleoside, while Fe3O4@TiGly had better enrichment and purification effect on phosphorylated polypeptide.
【學(xué)位授予單位】：武漢大學(xué)
【學(xué)位級別】：博士
【學(xué)位授予年份】：2016
【分類號】：TQ028
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